Coleman stole 110 bases in his debut season in 1985, easily setting a major league rookie record. Benny Kauff had had 75 steals as a rookie in the Federal League in 1914; Juan Samuel was considered MLB's rookie record holder with 72 steals in 1984. To date, the 110 steals are the third-highest in Major League history, after Rickey Henderson's 130 in 1982 and Lou Brock's 118 in 1974. Coleman stole over 100 bases in each of the following two seasons as well, making him the only player in the 20th century to post three consecutive seasons of 100 or more steals and the first player in Major League history to steal 100 bases in the first three seasons of their career. By the end of only his second year, his 217 stolen bases were second in Cardinal history behind Lou Brock's 888, just ahead of the 203 by Jack Smith.[2] Before signing as a free agent with New York, Coleman led the National League in stolen bases in every season he played with the Cardinals (1985-1990), becoming one of just four players ever to lead his league in six consecutive seasons. The other players to accomplish this feat are Henderson, Luis Aparicio, and Maury Wills. Coleman, Henderson, Wills and Brock are the only players to steal 100 bases in a season. Only Coleman and Henderson have three different 100-steal seasons to their credit, and only Coleman reached the total in three consecutive years.

As the leadoff hitter and baserunning sparkplug for St. Louis, Coleman helped the team reach the 1985 playoffs. But he suffered a freak injury prior to the fourth game of the National League Championship Series, when the automatic tarpaulin at Busch Stadium rolled over his leg during routine stretching exercises. The injury sidelined him for the rest of the postseason, and the Cardinals eventually lost a seven-game World Series to Kansas City.[3] Following the season, Coleman became the fourth-ever unanimous selection for the NL Rookie of the Year Award.

He offended many baseball fans, the press and many African Americans in 1985 when he declared "I don't know nothin' about him. Why are you asking me about Jackie Robinson?"[4] Responding to Coleman, Rachel Robinson, Jackie Robinson's widow said, "I hope somehow he'll learn and be embarrassed by his own ignorance."

Coleman compiled the best season of his major league career in 1987, when he posted a .289 batting average and a .363 on-base percentage while totaling 180 hits, 109 stolen bases, and 121 runs scored. He stole second and third base in the same inning 13 times that year. Coleman played in the World Series that year, the only one he would appear in. In June, he recorded his 500th stolen base in just his 804th game, the fewest that any player has needed to reach that milestone.

In 1989, Coleman compiled a streak of 50 successful stolen bases without being caught stealing, before it was broken on July 28 when he was thrown out by Montreal Expos catcher Nelson Santovenia in a game at Olympic Stadium.[5] The next night, July 29, 1989, Coleman was called out twice for interference on the base paths - first by using his hands to hit a ball foul, and then tugging at the uniform of Expos second baseman Damaso Garcia to break up a double play.

Coleman left for the Mets after the 1990 season via free agency, signing a four-year, $11.95 million contract. However, his career took a quick downward spiral. He missed 215 games (out of a possible 486) due to numerous injuries and suspensions. Coleman was one of three Met players named in a complaint filed by a 31-year-old woman in Florida, although prosecutors did not pursue charges in the case. His base-stealing strategy became increasingly suspect; he often ignored or misinterpreted his coaches' signs on the basepaths. He was also very difficult to get along with. He got into an ugly argument with coach Mike Cubbage at the tail end of his first season which was a factor in manager Bud Harrelson's ouster. In September 1992, he got into a fight with Harrelson's successor, Jeff Torborg, and was suspended without pay for the rest of the season. The Mets seemingly had enough and tried to trade him, but there were no takers. In April 1993, Coleman injured Dwight Gooden's arm by recklessly swinging a golf club in the clubhouse. Three months later, Coleman was charged with endangerment when he threw a lit firecracker into a crowd of baseball fans waiting for autographs in the Dodger Stadium parking lot. The explosion injured three children, including a two-year-old, Amanda Santos. He was sentenced to 200 hours of community service for the incident. The Mets placed him on paid administrative leave—in effect, a suspension with pay. On August 26, the Mets announced that as part of a general housecleaning of the clubhouse, Coleman would not return in 1994. Manager Dallas Green said that while Coleman had played well (when he suited up), he didn't think Coleman had the "head and heart and belly" he wanted to see on the team.[6]

He recorded 76 steals in 179 games as a Royal before being traded to the Seattle Mariners in mid-1995. 1996 found Coleman with the Cincinnati Reds, where he was ineffective. Released by the team in June, he signed with the California Angels but never played a game for the team. Coleman's final season in the major leagues came in 1997 with the Detroit Tigers, where he again received limited playing time and little success on the basepaths or elsewhere.

Coleman attempted a comeback with the St. Louis Cardinals in 1998 and hit over .300 in spring training, but did not earn a spot on the opening day roster. He was assigned to the AAA Memphis Redbirds, where he continued to play well, stealing eight bases and hitting .316 with an on-base percentage of .395 in 20 games as the club's regular left fielder and leadoff man. However, after failing to receive a promotion to St. Louis, Coleman elected to retire in May 1998, finishing his professional career with 752 stolen bases.

Coleman currently ranks sixth in all-time career steals in the major leagues, with 752. He also ranks 40th all-time in career stolen base percentage among all players with 80 or more attempts, at 80.947%.